Scale-Up of Room-Temperature Constructive Quantum Interference from Single Molecules to Self-Assembled Molecular-Electronic Films.
Scale-Up of Room-Temperature Constructive Quantum Interference from Single Molecules to Self-Assembled Molecular-Electronic Films.
复制标题
从单分子到自组装分子电子膜的室温构建量子干扰的扩展。
DOI：
10.1021/jacs.9b13578
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发表时间：
2020-05-13
影响因子：
15
通讯作者：
Lambert CJ
中科院分区：
文献类型：
--
作者：
Wang X;Bennett TLR;Ismael A;Wilkinson LA;Hamill J;White AJP;Grace IM;Kolosov OV;Albrecht T;Robinson BJ;Long NJ;Cohen LF;Lambert CJ
由量子干涉(QI)控制其室温输运性质的自组装分子电子薄膜的实现，是量子干涉效应从单分子到平行分子阵列放大的关键一步。最近，破坏性的QI(DQI)对自组装单分子膜(SAM)电导的影响被研究。在这里，我们通过实验和理论相结合的研究，展示了不同形式的构造性QI(CQI)在通过自组装膜的跨平面传输中的化学控制，并评估了其对自组装膜跨平面热电的影响。众所周知，单分子的电导可以通过化学改变其与外部电极的连接性来以确定性的方式进行控制。在这里，通过使用合成方法来改变芳香蒽核周围末端锚基的连接性，并通过形成所得到的分子的自组装膜，我们清楚地证明了CQI的这一特征可以被翻译成金上的SAM分子膜。结果表明，由具有两种不同连接性的蒽基分子形成的垂直分子结的电导相差约16倍，这与基于核心内CQI效应的电导比的理论预测一致。我们还证明，对于带有硫醚锚基的分子，这种薄膜的塞贝克系数与连接性有关，适当选择连接性可以使∼提高50%。在SAM中，QI及其对热电的影响的这一演示代表着向用于未来热电和分子规模电子应用的功能性超薄膜器件迈出的关键一步。
The realization of self-assembled molecular-electronic films, whose room-temperature transport properties are controlled by quantum interference (QI), is an essential step in the scale-up of QI effects from single molecules to parallel arrays of molecules. Recently, the effect of destructive QI (DQI) on the electrical conductance of self-assembled monolayers (SAMs) has been investigated. Here, through a combined experimental and theoretical investigation, we demonstrate chemical control of different forms of constructive QI (CQI) in cross-plane transport through SAMs and assess its influence on cross-plane thermoelectricity in SAMs. It is known that the electrical conductance of single molecules can be controlled in a deterministic manner, by chemically varying their connectivity to external electrodes. Here, by employing synthetic methodologies to vary the connectivity of terminal anchor groups around aromatic anthracene cores, and by forming SAMs of the resulting molecules, we clearly demonstrate that this signature of CQI can be translated into SAM-on-gold molecular films. We show that the conductance of vertical molecular junctions formed from anthracene-based molecules with two different connectivities differ by a factor of approximately 16, in agreement with theoretical predictions for their conductance ratio based on CQI effects within the core. We also demonstrate that for molecules with thioether anchor groups, the Seebeck coefficient of such films is connectivity dependent and with an appropriate choice of connectivity can be boosted by ∼50%. This demonstration of QI and its influence on thermoelectricity in SAMs represents a critical step toward functional ultra-thin-film devices for future thermoelectric and molecular-scale electronics applications.
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影响因子：
3.3
作者：
Gomar-Nadal, E;Ramachandran, GK;Lindsay, SM
通讯作者：
Lindsay, SM
利用破坏性γ干扰全面抑制单分子电导
影响因子：
64.8
作者：
Garner, Marc H.;Li, Haixing;Solomon, Gemma C.
通讯作者：
Solomon, Gemma C.
影响因子：
6.7
作者：
Herrer, L.;Ismael, A.;Cea, P.
通讯作者：
Cea, P.
影响因子：
16.6
作者：
Arroyo, Carlos R.;Tarkuc, Simge;van der Zant, Herre S. J.
通讯作者：
van der Zant, Herre S. J.
影响因子：
38.3
作者：
Guedon, Constant M.;Valkenier, Hennie;van der Molen, Sense Jan
通讯作者：
van der Molen, Sense Jan